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Roll Tide from Crimson Tide is most approriate for Command and generally I play Hans Zimmer soundtracks from Spotify when playing. They have proper seriousness for Command. Would post direct link to "Roll Tide", but forum software says I don't have enough posts.

Blues guitar is my usual go to. Stevie Ray Vaughn, Albert King, Robert Cray, Buddy Guy, B.B. King, et al.

Usually something ambient, dark and ominous like;
http://open.spotify.com/album/4rUUqub7MPuzNe1yEA17pr

With the sea-hag sounds running as well it gives a rather serious mood to the game.

Sound track from Medal of Honor: Allied assault (the first game). For some reason Neil Young also works with me...

I listen to all kinds of music playing Command, but my specially marked "playlist" is a mixture of orchestral march-styled music and dark, ambient electronic ones. (The latter is especially fitting in sub scenarios).

Ride of the Valkyries, ofcourse. On repeat.

Victory at Sea, (http://www.amazon.com/Victory-At-Sea-RE ... ory+at+sea)

Symphonic Battle Scenes (http://www.amazon.com/Symphonic-Battle- ... B000003G1X)

and anything by Al Stewart.

John Murphy's Sunshine and 28 Weeks Later soundtracks, Star Trek Into Darkness's soundtrack, Battlestar Galactica all seasons's soundtrack for my latest sessions. Of course, Basil Poledouris's Hunt for Red October soundtrack cannot remain unmentioned. Some Red Army's Choir also create a nice atmosphere.

Along that, I usually go for 19/20th century German, Czech, Russian composer's best off (TopClassicalMusic) or to contemporary "composers" (aka DJ) ala deadmau5 (thanks Baloogan!) and Skrillex.

Depending on the mood, I may prefer to play some progressive metal band ala Outrun the sunlight, Tool and so forth.

All that can be found on Youtube.

kexp.org or my rdio.com station.

I might be the odd one out here as when playing command I tend to avoid music with the proper "seriousness" as the OP says. Instead, I listen to La Cenerentola the 1981 version, which is a very weird subject matter for command, but it works for me [:D]